Process of oxidizing ammonia and catalytic bodies therefor.



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. I PROCESS OF OXIDIZING AMMONIA AND CATALYTIC BODIES THEREFQR.

the United States. or any of its ofiicers or employees in the prosecution of work for the United States, or by any other person in the United States, without the payment of any royalt thereon;

It is well own that when ammonia is mixed withan oxygen-containing gas and the mixture is heated to .a, suitable temperature, an oxidation and decomposition of the ammonia results with the formation of water and oxids of nitrogen. These reactions attain such a velocity in the presence of certain contact agents that the oxidation of ammonia has become a commercially important method of producing nitric acid. The ohject of this invention is to provide a contact agent which shows a high degree. of eifectiveness in promoting the above reaction, and which is in a large measure free from. certain defects which are encountered in the tlduse of the substances heretofore proposed.

Another object of my invention is to provide a material with which the catalyzer proper is mixed and on which it is carried in order that the activity of the catalyzer 40 may remain high and unim aired. These t5 ing ses are objects ll attain-by the use 0 the catalyzers and carriers hereinafter described, and m inventitn also comprises processes in whic mixtures of ammonia and oxygen-contain assed over mixtures of these catayzers an carriers or" over mixtures comprising any of them with other suitable carriers or catalyzers. I

l have discovered that lead oxid (P130) w is particularly efiective as a contact substance in the om'datiofi ofammonia. It has heretofore been proposed to employ for this urpose chemical compounds formed by eating lead oxid with magnesium ojxid or Specification of Letters Patent. Application filed Apri120, 191?. se n no. teat-cot.

.salt by heating, or by simply Patented dept. 4L, 1% t,

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with some other oxid, with which the lead oxid will unite to form a plumbate. Such plumbates form valuable catalyzers but their use is attended with certain disadvantages which I have sought to avoid. In forming the plumbates it is dificult to secure a mass of uniform chemical composition and physical characteristics, great care being requiredto avoid overheating. Furthermore, the finished plumbate has a stron tendency to become overheated when use and this overheatmg produces harmful results in the reaction products and in the catalyzer itself.

I have avoided these dificulties by using the lead oxid in uncombined form. ln order to produce the necessary porosity of the lead oxid, it has been found advisable to mix the same with a carrier, but for this catalyzer all the hitherto proposed carriers of which l am aware have proved unsuitable. This is because the lmown carriers, though unaffected by the catalyzers heretofore used, are

strongly attacked by the lead oxid at a dull red heat with the formation of plumbates, or glassy inactive masses. Thus, all silicates and all materials containingfree silica give lead-silica glasses with the lead oxid.

As a carrier for the lead oxid, I have found that bone-ash is admirably fitted. So

far as I am aware, this material has not been previously used for this purpose and it will be evident that it may also be advanta geously employed with other contact substances having a fluxing-action similar to i that of lead oxid. The lead oxid may be deposited on the bone ash by well @own methods, such as absorbing in the ash asolution of a soluble salt of lead, such as lead nitrate or lead acetate, drying the ash so impregnated and then decomposing the lead g a paste of the powdered oxid and bone ash and then drying and igniting the mixture at a low red heat. en properly prepared, the contact material has the homogeneous composition and finely-porous texture observrec able in bone ash cupels which have been used in the on fire assaying. size, the material is highly eficient as a con.- tabt body. 0

I do not limit my invention to. lead omd carried upon bone ash as it will be readily seen that other materials notattacked by cation of lead buttons in "W 1' crushed tothe-proper 1 ice lead'oxid at temperatures in the neighborvantage. ish Pat. 698 of 1902) has'mentioned that hood of 750 (3., such as c stalline alumina or carborundum may also e used with ad-' I am aware that Qstwald (Brit- 1 lead peroxid maybe used as a catalyzer in It may be carried upon asuitable inert ma- 4s cessive temperatures, and when such sinter-- by mixing the 7 any terial and in this case also bone ash is. very desirable as a carrier. The chromate may be deposited upon the carrier. by treating thelatter successlvely with solutions of lead salts and solutions ofcompounds of chromic acid, drying, heating, a and crushing. The contact material may also be prepared plowdered carrier and lead chromate as in t e case of lead oxid, or in other suitable way.

am aware that in the Bemchte .oler Deutchen Chem/580M Gesellschwft 4, 891 (1871 is an abstract of the specificationoi Britis atent to du Motay, 491 of 1871, and that said abstract states that the use of lead chromate as a catalyzer in the oxidation of ammonia is proposed in the patent specification, However, British Patent 491 of 1871 makes no mention of-lead chromate and so far as I am aware I am the first to propose the use of this compound, a When either lead oxid-or lead chromate is employed as the catalytic substance; practically complete oxidation of ammonla to oxlds of nitrogen may be obtained. Either the oxid or chromate may in certain casesv be usedjinlump form without a carrier, but in generalthe. use of a carrier with the catalyzer is} preferred. When 'used without a carrier, lead oxid is apt to sinter together unless great care is taken to guard against ex- 1n occurs, the individual pieces of the matenal fuse or weld together with a considerable impairment of the activity of the ma- .ture.

terial. 11m a suitable inert carrier is employed, t is undesirable result -is entirely avoided and in addition the effect of a given mass of the oxid is increased by causing it to expose a larger surface to the reacting mix- WhatI claim isi l. The process of. producing oxids of mtrogen whichrcomprises passing a mixture of ammonia and an oxygen-containing gas over a heated com osite, material comprising a water-insolub e lead compound and a carrier containing a phosphate oi .an alkali earth metal.

2. The-process of producing oxids of nitrogen which comprises passing a mixture of ammonia and an 0 gen-containing gas over a catalyzer ca 'e taining a phosphate of an alkali earth metal.

3. The rocess of producing oxids of ni-v trogen which comprises passing a mixture of ammonia-and an oxygen-contaming gas over a heated composite material comprising a on a material conleadcompound and a carrier contaming calcium hosphate.-

he recess of producing oxids of nitrogen whic comprises passing a mixture of ammonia and an, oxygen containing gas over a heated com oslte material comprlsmg a catalyzer and one ash as a carrier.

5. The process ofproducing oxids of nitrogen which comprises passing a mixture of ammonia and an oxygen-containmg gas over a heated composite material comprising lead chromate and a carrier which is not substantially chemically afiected by lead chromate at a temperature of 1000' deg. C.

6. The 'rocess of producing oxids of nitrogen wh1ch comprises passing a mixture of ammonia and an oxygen-containing gas over lead chromate carried-u n bone ash;

17. As a contact material or use in the oxidation of ammonia a composite material com rising lead chromate and a carrier whic is not substantially chemically afi'ected by lead chromate at a low red heat.

8.. As acontact material, lead chromate carried upon bone ash.

- ES LPAJRSONS. 

